We investigate the long-standing problem of hole localization at the Al impurity in quartz SiO<inf>2</inf>, using a relatively recent DFT hybrid-functional method in which the exchange fraction is obtained ab initio, based on an analogy with the static many-body COHSEX approximation to the electron self-energy. As the amount of the admixed exact exchange in hybrid functionals has been shown to be determinant for properly capturing the hole localization, this problem constitutes a prototypical benchmark for the accuracy of the method, allowing one to assess to what extent self-interaction effects are avoided. We obtain good results in terms of description of the charge localization and structural distortion around the Al center, improving with respect to the more popular B3LYP hybrid-functional approach. We also discuss the accuracy of computed hyperfine parameters, by comparison with previous calculations based on other self-interaction-free methods, as well as experimental values. We discuss and rationalize the limitations of our approach in computing defect-related excitation energies in low-dielectric-constant insulators.
Communication : Hole localization in Al-doped quartz SiO2 within ab initio hybrid-functional DFT / M. Gerosa, C. Di Valentin, C.E. Bottani, G. Onida, G. Pacchioni. - In: THE JOURNAL OF CHEMICAL PHYSICS. - ISSN 0021-9606. - 143:11(2015 Sep 21), pp. 111103.1-111103.5.
|Titolo:||Communication : Hole localization in Al-doped quartz SiO2 within ab initio hybrid-functional DFT|
|Parole Chiave:||DFT; ab-initio; defects; Oxydes; hybrid functionals|
|Settore Scientifico Disciplinare:||Settore FIS/03 - Fisica della Materia|
Settore CHIM/02 - Chimica Fisica
|Data di pubblicazione:||21-set-2015|
|Digital Object Identifier (DOI):||http://dx.doi.org/10.1063/1.4931405|
|Appare nelle tipologie:||01 - Articolo su periodico|